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Comet C/2017 K2 (Pan-STARRS) provided a rare opportunity to investigate the evolution of coma composition and outgassing patterns over a transitional heliocentric distance (Rh) range where activity drivers in comets are thought to change from "hypervolatile" (CO, CH4, C2H6, and/or CO2)-dominated to H2O-dominated. We performed high-resolution ( / ≈ 25,000–42,000), cross-dispersed, near-infrared spectroscopy of C/2017 K2 with iSHELL at the NASA Infrared Telescope Facility and NIRSPEC at the W. M. Keck II Observatory. We report gas rotational temperatures (Trot) and molecular production rates (Q; molecules per second) or upper limits for the "hypervolatile" species CH4, CO, and C2H6, together with less volatile ices (CH3OH, H2O, HCN, C2H2, NH3, and OCS) over a range of pre-perihelion distances, Rh = 3.15–2.35 au. We also report (or stringently constrain) abundance ratios (mixing ratios) of the targeted species with respect to CO, C2H6, and (when detected) H2O. All volatiles were enriched relative to water in C/2017 K2 when compared to their mean values among Oort Cloud comets, whereas abundances relative to C2H6 were consistent with their average values from other long-period comets.