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The synthesis and the magnetic properties of two new bimetallic chromium-vanadium ferrimagnets, compounds 1 and 2, are reported. They belong to a set of nonstoichiometric Prussian blue analogues C I y V-[Cr III (CN) 6 ] z ‚nH 2 O (C, alkali cation) with T C varying between 295 and 315 K (T C ) 310 K for 1 and 315 K for 2). They are obtained through mild chemistry from the molecular precursor [Cr III (CN) 6 ] 3and from vanadium V II salts. The synthetic conditions determine (i) the oxidation state of the vanadium (V II , V III , or V IV ), (ii) the stoichiometry, and (iii) hence the magnetic properties. The reported systems present a larger magnetization than the first reported V-Cr analogue (0.36N A β for 1 and 0.40N A β for 2). Furthermore, X-ray magnetic circular dichroism (XMCD) data demonstrate (i) the short-range antiferromagnetic coupling between the spins borne by the chromium(III) and vanadium ions and (ii) the reversal of the local magnetization on vanadium and chromium when changing the stoichiometry.