In this study we exploit the flexible nature of porous coordination polymers (PCPs) with integrated spin crossover (SCO) properties to manipulate the multistability of spin-state switching profiles. We previously reported the two-dimensional Hofmann-type framework [Fe(thtrz)(2)Pd(CN)4]center dot EtOH,H2O (1 center dot EtOH,H2O), N-thiophenylidene-4H-1,2,4-triazol-4-amine), displaying a distinctive two-step SCO profile driven by extreme elastic frustration. Here, we reveal a reversible release mechanism for this elastic frustration via stepwise guest removal from the parent phase (1 center dot EtOH,H2O -> 1 center dot H2O -> 1 center dot empty set). Parallel variable temperature structural and magnetic susceptibility measurements reveal a synergistic framework flexing and "on-off" switching of multistep SCO character concomitant with the onset of guest evacuation. In particular, the two-step SCO properties in 1 center dot EtOH,H2O are deactivated such that both the partially solvated (1 center dot H2O) and desolvated (1 center dot empty set) phases show abrupt and hysteretic one-step SCO behaviors with differing transition temperatures (1 center dot H2O: T-1(/2)down arrow: 215 T-1(/2)up arrow: 235 K; 1 center dot empty set: T-1(/2)down arrow: 170 T-1(/2)up arrow: 182 K). This "on-off" elastic frustration switching is also reflected in the light-induced excited spin state trapping (LIESST) properties of 1 center dot EtOH,H2O and 1 center dot empty set, with nonquantitative (ca. 50%, i.e., LS <--> 1:1 HS:LS) and quantitative (ca. 100%, LS <--> HS) photoinduced spin state conversion achieved under light irradiation (510 nm at 10 K), respectively. Conversely, the two-step SCO properties are retained in the water saturated phase 1 center dot 3H(2)O but with a subtle shift in transition temperatures. Comparative analysis of this and related materials reveals the distinct roles that indirect and direct guest interactions play in inducing, stabilizing, and quantifying elastic frustration and the importance of lattice flexibility in these porous framework architectures.