Magnetically bistable solid solutions of Prussian blue analogues with chemical formulas of K αNi 1-xCo x[Fe(CN) 6] β•nH 2O (Ni 1-xCo xFe) and K αCo γ[Fe(CN) 6] y[Cr(CN) 6] 1-y•nH 2O (CoFe yCr 1-y) have been synthesized and studied using mass spectrometry, Mössbauer spectroscopy, X-ray diffraction, temperature-dependent infrared spectroscopy, and dc magnetometry. These compounds provide insight into interfaces between the photomagnetic Co-Fe Prussian blue analogue and the high-T C Ni-Cr Prussian blue analogue that exist in high-T C photomagnetic heterostructures. This investigation shows that the bistability of Co-Fe is strongly modified by metal substitution, with Ni 1-xCo xFe stabilizing high-spin cobalt-iron pairs and CoFe yCr 1-y stabilizing low-spin cobalt-iron pairs, while both types of substitution cause a dramatic decrease in the bistability of the material.