In their article, Zhang et al. [Phys. Rev. B 86, 024516 (2012)] present a remarkable result for ${A}_{x}{(S)}_{y}\mathrm{TiNCl}$ compounds ($\ensuremath{\alpha}$-phase TiNCl partially intercalated with alkali $A$ and optionally co-intercalated molecular species $S$), finding the superconducting transition temperature ${T}_{c}$ scales with ${d}^{\ensuremath{-}1}$, where the spacing $d$ between TiNCl-layered structures depends on intercalant thickness. Recognizing that this behavior indicates interlayer coupling, Zhang et al. cite, among other papers, the interlayer Coulombic pairing mechanism picture [Harshman et al., J. Phys.: Condens. Matter 23, 295701 (2011)]. This Comment shows that superconductivity occurs by interactions between the chlorine layers of the TiNCl structure and the layers containing ${A}_{x}$, wherein the transverse ${A}_{x}\text{\ensuremath{-}}\mathrm{Cl}$ separation distance $\ensuremath{\zeta}$ is smaller than $d$. In the absence of pair-breaking interactions, the optimal transition temperature is modeled by ${T}_{c0}\ensuremath{\propto}{(\ensuremath{\sigma}/A)}^{1/2}{\ensuremath{\zeta}}^{\ensuremath{-}1}$, where $\ensuremath{\sigma}/A$ is the fractional charge per area per formula unit. Particularly noteworthy are the rather marginally metallic trends in resistivities of ${A}_{x}{(S)}_{y}\mathrm{TiNCl}$, indicating high scattering rates, which are expected to partially originate from remote Coulomb scattering (RCS) from the ${A}_{x}$ ions. By modeling a small fraction of the RCS as inducing pair breaking, taken to cut off exponentially with $\ensuremath{\zeta}$, observations of ${T}_{c}<{T}_{c0}$ are quantitatively described for compounds with $\ensuremath{\zeta}<4\phantom{\rule{0.16em}{0ex}}\AA{}$ and ${T}_{c}\ensuremath{\approx}{T}_{c0}$ for $\mathrm{N}{\mathrm{a}}_{0.16}{(S)}_{y}\mathrm{TiNCl}$ with propylene carbonate and butylene carbonate co-intercalants for which $\ensuremath{\zeta}>7\phantom{\rule{0.16em}{0ex}}\AA{}$. Since a spatially separated alkali-ion layer is not formed in $\mathrm{L}{\mathrm{i}}_{0.13}\mathrm{TiNCl}$, the observed ${T}_{c}$ of 5.9 K is attributed to an intergrowth phase related to TiN $({T}_{c}=5.6\phantom{\rule{0.16em}{0ex}}\mathrm{K})$.