Molecular fragmentation methods have revolutionized quantum chemistry. Here, we use a graph-theoretically generated molecular fragmentation method, to obtain accurate and efficient representations for multidimensional potential energy surfaces and the quantum time-evolution operator, which plays a critical role in quantum chemical dynamics. In doing so, we find that the graph-theoretic fragmentation approach naturally reduces the potential portion of the time-evolution operator into a tensor network that contains a stream of coupled lower-dimensional propagation steps to potentially achieve quantum dynamics with reduced complexity. Furthermore, the fragmentation approach used here has previously been shown to allow accurate and efficient computation of post-Hartree-Fock electronic potential energy surfaces, which in many cases has been shown to be at density functional theory cost. Thus, by combining the advantages of molecular fragmentation with the tensor network formalism, the approach yields an on-the-fly quantum dynamics scheme where both the electronic potential calculation and nuclear propagation portion are enormously simplified through a single stroke. The method is demonstrated by computing approximations to the propagator and to potential surfaces for a set of coupled nuclear dimensions within a protonated water wire problem exhibiting the Grotthuss mechanism of proton transport. In all cases, our approach has been shown to reduce the complexity of representing the quantum propagator, and by extension action of the propagator on an initial wavepacket, by several orders, with minimal loss in accuracy.