By this result claimed on the nlab the free forgetful adjunction $F \dashv U$ between abelian groups and sets gives rise to a biadjunction(?) $\overline{F} \dashv \overline{U}$ between the bicategories $\mathsf{Ab}-\mathsf{Cat}$ and $(\mathsf{Set}-)\mathsf{Cat}$. My understanding is that $\overline{F}$ takes an ordinary category $\mathsf{C}$ and constructs an $\mathsf{Ab}$-enriched category $\overline{F}(\mathsf{C})$ which has the same objects as $\mathsf{C}$ but $\operatorname{Hom}_{\overline{F}(\mathsf{C})}(x, y) = F(\operatorname{Hom}_{\mathsf{C}}(x, y))$
whereas $\overline{U}$ takes an $\mathsf{Ab}$-enriched category $\mathcal{S}$ and constructs an ordinary category $\overline{U}(\mathcal{S})$ which has the same objects as $\mathcal{S}$ but $\operatorname{Hom}_{\overline{U}(\mathcal{S})}(x, y) = U(\operatorname{Hom}_{\mathcal{S}}(x, y))$ and we have pseudonatural adjoint equivalences $\mathsf{Ab-Fun}(\overline{F}(\mathsf{C}), \mathcal{S}) \simeq \operatorname{Fun}(\mathsf{C}, \overline{U}(\mathcal{S}))$.
In particular the $\mathsf{Ab}$-enriched category $+\Delta \stackrel{\text{def}}= \overline{F}(\Delta)$ has the structure of a mapping out property $\mathsf{Ab-Fun}(+\Delta^{\mathrm{op}}, \mathcal{M}) \simeq \operatorname{Fun}(\Delta^{\mathrm{op}}, \overline{U}(\mathcal{M})) = s\overline{U}(\mathcal{M})$. This is classified by a simplicial object of $+\Delta^{\mathrm{op}}$, dually a cosimplicial object of $+\Delta$, which can be calculated as the unit of the $2$-adjunction $\overline{F} \dashv \overline{U}$ at component $\Delta$, which is the identity on objects and the unit of $F \dashv U$ on $\operatorname{Hom}$-sets, i.e. the identity on objects and the inclusion of basis elements on morphisms. So the cosimplicial object $A$ of $+\Delta$ has $A_n = [n]$, and the coface maps $d^i : A_n \to A_{n-1}$ are defined on basis elements by $d^i(f) = \delta^i(f)$ and extended additively (similarly for codegeneracy maps).
Now because $\mathsf{Ab}$ is a nice enough enriching category (cosmos I think?) we can promote the ordinary category $\mathsf{Ab-Fun}(\mathcal{R}, \mathcal{S})$ to an $\mathsf{Ab}$-enriched category $+\mathsf{Fun}(\mathcal{R}, \mathcal{S})$ with $\overline{U}(+\mathsf{Fun}(\mathcal{R}, \mathcal{S})) = \mathsf{Ab-Fun}(\mathcal{R}, \mathcal{S})$. This is just "remembering" that we can add and subtract morphisms between abelian groups.
The category of enriched presheaves is $\mathsf{Mod}(\mathcal{R}) \stackrel{\text{def}}= +\mathsf{Fun}(\mathcal{R}^{\mathrm{op}}, \mathsf{Ab})$ is the free $\mathsf{Ab}$-cocompletion of $\mathcal{R}$. Note $\mathsf{Mod}(+\Delta) = s\mathsf{Ab}$.
Connective chain complexes of abelian groups are also the category of modules over an $\mathrm{Ab}$-enriched category $\mathcal{R}$. This category is $\mathcal{R} = \overline{F}(\mathbb{N}^{\leq})/J$, where $\mathbb{N}^{\leq}$ is the poset category of the nonnegative integers and $J$ is the ideal generated by all morphisms of the form $d_n^2$, where $d_n$ is the basis element corresponding to the element of $\mathrm{Hom}_{\mathbb{N}^{\leq}}(n, n + 1)$. So the subgroup of $\mathrm{Hom}_{\mathbb{N}^{\leq}}(n, m)$ given by $J$ is $0$ if $m = n + 1$ or $m = n$ and is the entire subgroup otherwise. More concretely $\mathcal{R}$ has objects the natural numbers and $$\operatorname{Hom}_{\mathcal{R}}(n, m) = \begin{cases} F(\{d\}) &\text{ if } m = n + 1 \\ F(\{\mathrm{id}_n\}) &\text{ if } m = n \\ 0 &\text{ otherwise.} \end{cases}$$
The dual of the standard proof that the differential of the Moore complex squares to $0$ proves that we have a well defined (additive) functor $M' : \mathcal{R} \to \Delta+$, sending $n$ to $[n]$ and sending the differential to the alternating sum of coface maps. Composing this with the enriched Yoneda embedding gives rise to an adjunction between the essentially unique $\mathsf{Ab}$-enriched colimit preserving extension of $y \circ M'$, a functor $\mathsf{Mod}(\mathcal{R}) = \mathsf{Ch}^+(\mathbb{Z}) \to s\mathsf{Ab}$, and the nerve of $y \circ M'$, a functor $s\mathsf{Ab} \to \mathsf{Ch}^+(\mathbb{Z})$. This nerve sends a simplicial abelian group to its alternating face map complex, i.e. is the Moore complex functor. This "explains" the left adjoint of the Moore complex functor. But also because the functor $y\circ M'$ is valued in projective objects (representables) the nerve $M$ automatically preserves colimits (one can see this from the defintion of the nerve and the fact that preservation of colimits can be checked after evaluating at each object). Hence it has a further right adjoint, although I still don't know a better direct description of this adjoint.
It's interesting to me that the Moore complex arises from a functor of small categories $\mathcal{R} \to +\Delta$ while the better behaved normalized Moore complex requires a cosimplicial object in the large category functor $\mathsf{Ch}^+(\mathbb{Z})$. This cosimplicial chain complex is in degree $n$ the the complex which in degree $m$ is the free abelian group on injections $[m] \hookrightarrow [n]$ and whose differential is the alternating sum of the precompositions with coface maps. The coface maps of this cosimplicial object postcompose with the coface maps in the simplex category and the codegeneracy maps are all zero. My two thoughts here are that we didn't actually need the whole category $\mathsf{Ch}^+(\mathbb{Z})$, the complexes involved are all perfect, and that I should think about the semisimplicial version of Dold Kan.