Reaction of 4-methyl-pyridine N-oxide and Co(NCS)2 in ethanol as solvent accidentally leads to the formation of single crystals of Co(NCS)2(4-methyl-pyridine N-oxide)(ethanol) or [Co(NCS)2(C6H7NO)(C2H6O)] n . The asymmetric unit of the title compound consists of one CoII cation, two crystallographically independent thio-cyanate anions, one 4-methyl-pyridine N-oxide coligand and one ethanol mol-ecule on general positions. The cobalt cations are sixfold coordinated by one terminal and two bridging thio-cyanate anions, two bridging 4-methyl-pyridine N-oxide coligands and one ethanol mol-ecule, with a slightly distorted octa-hedral geometry. The cobalt cations are linked by single μ-1,3(N,S)-bridging thio-cyanate anions into corrugated chains, that are further connected into layers by pairs of μ-1,1(O,O)-bridging 4-methyl-pyridine N-oxide coligands. The layers are parallel to the bc plane and are separated by the methyl groups of the 4-methyl-pyridine N-oxide coligands. Within the layers, intra-layer hydrogen bonding is observed.