AbstractLarge, open‐gate transistors made from metal nanoparticle arrays offer possibilities to build new electronic devices, such as sensors. A nanoparticle necklace network (N3) of Au particles from 300 K to cryogenic temperatures exhibit a nonohmic I–Vd behavior, I ≈ (Vd–VT)ζ, where VT is a conduction gap and ζ is a constant critical exponent. The conduction gap in N3, made from disordered networks of 1D chains of 10 nm diameter Au particles exhibits room temperature (RT) gating. Although the I–Vd behavior at RT is identical to Coulomb blockade, the conduction is modulated by field‐assisted tunneling exhibiting classical critical behavior. In this study, based on three results, invariance of VT on gating, invariance of VT on temperature, and zero–bias conductance, a sharp transition temperature at ≈140 K is discovered where the conduction mechanism switches from Coulomb blockade to classical critical percolation behavior. The N3 architecture allows the reconciliation of the Coulomb blockade versus activation process as a sharp thermal transition to serve as a model system to study the exotic behavior in nanogranular‐metallic materials. The novel global critical behavior to local Coulomb blockade governed transition in these N3 architectures may potentially lead to novel sensors and biosensors.