Two mononuclear octahedral Co(II) complexes, [Co(L)X2] (L = 1-(prop-2-en-1-yl)-1H-imidazole, X = NCS- (1) and NCSe- (2)), have been synthesized and characterized. The central Co(II) ions in two complexes adopt an octahedral geometry, coordinated by four N atoms from the ligand and two N atoms from the anion. Direct-current magnetic data revealed large easy-plane magnetic anisotropy in both 1 and 2. Dynamic magnetic measurements demonstrated that 1 and 2 display field-induced slow magnetic relaxation. For 1 and 2, the Raman mechanism is found to the dominant process in the whole temperature range. Compared to 1, the magnetic relaxation of 2 is faster, likely due to the presence of the hydrogen bonding system in 2.