Temperature dependencies of dielectric permittivity and loss tangent (at frequencies 0.1-200 kHz) together with thermally stimulated depolarization currents, magnetization, and Mössbauer spectra of ceramic solid solutions Co 1−x Ni x Cr 2 O 4 (x = 0, 0.2, 0.4, 0.6, 1.0) are studied at temperatures from 80 to 350 K. We find evidence of two reversible phase transitions located at T 1 and T 2 (220 and 245 K, respectively, for x = 0.2), of occurrence of pyroelectric properties below T 2 , as well as of a phase transition to magnetically ordered state of ferrimagnetic type (below 86 K for x = 0.2). The obtained results evidence that the compounds possess, additionally to magnetic, ferroelectric properties and are thus new members in the family of multiferroics.Spinel compounds with Jahn-Teller cations reveal structural phase transitions caused by removal of the orbital degeneracy leading to ordering of the d orbitals and to lowering of the crystal lattice symmetry. As a result, some low-symmetry phases become polar and reveal multiferroic properties. [1][2][3][4][5][6][7][8][9][10][11][12] Most detailed studies of such multiferroicity were performed for magnetite (Fe 2+ Fe 2 3+ O 4 ) whose low-symmetry phase is monoclinic (Cc) 5 ; here, switching between magnetic and electrical orderings can be driven by both magnetic and electric fields. 1-4 Recently, similar studies were performed also on chromites, like CoCr 2 O 4 . 7-12 Cobalt CoCr 2 O 4 and nickel NiCr 2 O 4 chromites belong to the spinel family with the general formula AB 2 O 4 in which Co 2+ (3d 7 ) or Ni 2+ (3d 8 ) bivalent cations occupy tetrahedrally coordinated by oxygen A positions and the Cr 3+ trivalent cations-octahedral positions. 6-14 These compounds crystallize, at rather high temperatures, into a cubic phase with the space group F d3m (No. 227). When lowering the temperature, the symmetry of the nickel chromite decreases to tetrahedral at 320 K, while the cobalt chromite remains cubic down to 10 K. 7-19 In NiCr 2 O 4 , the phase transition between cubic and tetragonal states (the C-T transition) is of the first-order type, near to second-order type phase transition, with the tetragonal form relating to ferroelastics. It is driven by a cooperative Jahn-Teller effect in the array of Ni 2+ cations in tetrahedral positions [for the Cr 3+ (3d 3 ) cations the Jahn-Teller effect in the octahedral crystal field is not observed]. In ACr 2 O 4 , the transition into the ferrimagnetic state takes place at T N = 93 K for A = Co and at T N = 70 К for A = Ni. 6,9,11,[20][21][22] In spite of the fact that the considered complex oxides reveal intriguing elastic, electrical, magnetic, catalytic, and other physical properties and attract much attention, 1-25 there is practically no data in the literature on their dielectric characteristics. In this paper we present our results on the first measurements of the temperature-frequency behavior of the complex dielectric permittivity ε * = ε 1 + iε 2 , loss tangent tgδ = ε 2 /ε 1