The invention relates to a Co-bis-imidazolyl metal frame compound, a preparation method and application thereof. The metal frame compound has a chemical formula of {Co2(1, 2-BIB)(BTC)}n, wherein 1, 2-BIB is 1, 2-methylene imidazolyl benzene, and BTC is deprotonated 1, 2, 4, 5-benzenetetracarboxylicacid. The compound provided by the invention has the characteristics of simple and easily operated preparation method, low cost, stability below 230DEG C, and very strong third-order nonlinear optical saturated absorption performance, with a third-order nonlinear saturated absorption coefficient beta of -4.55*10<-6>m/W and a third-order nonlinear polarizability x<(3)> of 7.33*10<-8>es, the material can be widely applied to in laser pulse compression (Q switch and mode locking) and other fields.