In this paper, we present a study of the electron spin resonance (ESR) of nanoparticles (NPs) of Cu1 xFexCr2Se4 chalcogenides with x = 0, 0.2, and 0.4. NPs were synthesized via the thermal decomposition of metal chloride salts and selenium powder in a high-temperature organic solvent. According to the XRD and HRTEM data, the NPs were single crystalline nearly hexagonal plates with the structure close to CuCr2Se4 (Fd-3m, a = 10.337 Å). For x = 0 and 0.2, the NPs tend to form long stacks consisting of the plates ‘‘face to face” attached to each other due to the magnetostatic interparticle interaction. Only separate NPs were observed in the case of x = 0.4. Peculiarities were revealed in the ESR temperature behavior for the
NPs with x = 0 and 0.2 consistent with the features in the temperature dependences of the NPs magnetization. The non-monotonous dependence of the resonance field Hres on the temperature with a kink near 130 K and the energy gap in the resonance spectrum depending on the type of nanoparticle compacting are the distinct peculiarities. One of the main factors is discussed in order to explain the peculiarities: the coexistence of two types of anisotropy in the Cu1 xFexCr2Se4 NPs, in-plain shape anisotropy and magnetocrystalline anisotropy with four easy axes, which increases strongly with the temperature decrease.