Photomagnetic compounds are usually achieved by assembling preorganized individual molecules into rationally designed molecular architectures via the bottom-up approach. Here we show that a magnetic response to light can also be enforced in a nonphotomagnetic compound by applying mechanical stress. The nonphotomagnetic cyano-bridged Fe-II-Nb-IV coordination polymer {[Fe-II(pyrazole)(4)](2)[Nb-IV(CN)(8)].4H(2)O}(n) (FeNb) has been subjected to high-pressure structural, magnetic and photomagnetic studies at low temperature, which revealed a wide spectrum of pressure-related functionalities including the light-induced magnetization. The multifunctionality of FeNb is compared with a simple structural and magnetic pressure response of its analog {[Mn-II(pyrazole)(4)](2)[Nb-IV(CN)(8)].4H(2)O}(n) (MnNb). The FeNb coordination polymer is the first pressure-induced spin-crossover photomagnet.