A nickel(II) complex (1) of N,N'-bis(2,6-diisopropylphenyl)-2,6-pyridinedicarboxamido (L) ligand was examined for catalytic coupling of Grignard reagents with the C-H bond of oxygen containing heterocyclic compounds such as tetrahydrofuran and furan. The nickel(II) complex showed excellent activity in catalyzing C-H activation and further coupling with various Grignard reagents. The effective activation of the C-H bond proceeded under ambient reaction conditions with a short reaction time (1-2 h). The catalyst (1) displays high turnover frequency of 4,130 h(-1) with catalyst loading as low as 0.01 mol%. This catalytic route could prove to be an efficient mode of activation of sp(3) and sp(2) C-H bonds in various heterocycles for the preparation of synthetically and pharmaceutically relevant molecules.