A criterion method of GCCS (Globally Complete Chaos Synchronization) for three-node VCSEL (Vertical Cavity Surface Emitting Laser) networks with delay coupling is provided, including steps of: providing a delay-coupled VCSEL network consisting of three identical units and dynamic equations of the VCSEL network; providing assumptions of an outer-coupling matrix and a unitary matrix under the dynamic equations of the VCSEL network; in the three-node VCSEL network, determining rate equations of i-VCSEL, determining dynamic equations of a synchronization manifold, and determining a master-stability equation; calculating three maximum Lyapunov exponents; determining a stability of a synchronization state of the three-node VCSEL network, and determining whether the synchronization manifold of the VCSEL network is a chaotic waveform. Through a master-stability function, the method for determining whether the GCCS is achieved among all node lasers is provided, which solves a difficult problem of GCCS criterion for the VCSEL networks.