Zn_1−xCo_xO (x==0.05, 0.10, 0.15) nanoparticles have been synthesized by an alternative wet-chemical synthesis route using the SimAdd technique. The as-obtained powders were investigated by FT-IR spectroscopy, X-ray diffraction and thermal analysis correlated with evolved gas analysis (TG–DTA–FT-IR) in order to determine their chemical nature, crystalline structure and to establish the decomposition sequences. The precipitates are generally amorphous, but low-intensity reflection peaks assigned both to the zinc oxalate dihydrate, and zinc hydroxide can be observed in the recorded patterns, indicating that hydroxy-oxalate precipitates were obtained. The structure, morphology and magnetic properties of the thermally treated samples have been investigated by X-ray diffraction, FT-IR, HRTEM, SAED, UV–vis and EPR. XRD studies reveal a hexagonal wurtzite-type structure for all Zn_1−xCo_xO samples. TEM investigations show particle size between 28 and 37 nm, with spherical and polyhedral shapes and with tendency to form aggregates. The presence of a Co₃O₄ secondary phase was evidenced by XRD, UV–vis and EPR for the Zn_0.85Co_0.15O sample. The ferromagnetic behavior of the samples was revealed. The paper highlights that by varying the cobalt concentration it is possible to modulate the structural, morphological, optical and magnetic properties.