We present the mass excesses of Cr59-64, obtained from recent time-of-flight nuclear mass measurements at the National Superconducting Cyclotron Laboratory at Michigan State University. The mass of Cr64 is determined for the first time, with an atomic mass excess of -33.48(44) MeV. We find a significantly different two-neutron separation energy S2n trend for neutron-rich isotopes of chromium, removing the previously observed enhancement in binding at N=38. Additionally, we extend the S2n trend for chromium to N=40, revealing behavior consistent with the previously identified island of inversion in this region. We compare our results to state-of-the-art shell-model calculations performed with a modified Lenzi-Nowacki-Poves-Sieja interaction in the fp shell, including the g9/2 and d5/2 orbits for the neutron valence space. We employ our result for the mass of Cr64 in accreted neutron star crust network calculations and find a reduction in the strength and depth of electron-capture heating from the A=64 isobaric chain, resulting in a cooler than expected accreted neutron star crust. This reduced heating is found to be due to the >1-MeV reduction in binding for Cr64 with respect to values from commonly used global mass models.