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 FeII–NbIV coordination polymer {[FeII(pyrazole)4]2[NbIV(CN)8]·4H2O}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 {[MnII(pyrazole)4]2[NbIV(CN)8]·4H2O}n (MnNb). The FeNb coordination polymer is the first pressure-induced spin-crossover photomagnet.