Nanosized samples of the cubic thiospinel FeCr2S4 were synthesized by ball milling of FeS and Cr2S3 precursors followed by a distinct temperature treatment between 500 and 800 °C. Depending on the applied temperature, volume weighted mean (Lvol) particle sizes of 56 nm (500 °C), 86 nm (600 °C), and 123 nm (800 °C) were obtained. All samples show a transition into the ferrimagnetic state at a Curie temperature TC of ∼ 167 K only slightly depending on the annealing temperature. Above TC, ferromagnetic spin clusters survive and Curie–Weiss behavior is observed only at T ≫ TC, with T depending on the heat treatments and the external magnetic field applied. Zero-field-cooled and field-cooled magnetic susceptibilities diverge significantly below TC in contrast to what is observed for conventionally solid-state-prepared polycrystalline samples. In the low-temperature region, all samples show a transition into the orbital ordered state at about 9 K, which is more pronounced for the samples heated to higher temperatures. This observation is a clear indication that the cation disorder is very low because a pronounced disorder would suppress this magnetic transition. ... mehrThe unusual magnetic properties of the samples at low temperatures and different external magnetic fields can be clearly related to different factors like structural microstrain and magnetocrystalline anisotropy.