We propose a novel low temperature annealing method for selective crystallization of gold thin films. Our method is based on a non-melt process using highly overlapped ultrashort laser pulses at a fluence below the damage threshold. Three different wavelengths of a femtosecond laser with the fundamental (1030 nm), second (515 nm) and third (343 nm) harmonic are used to crystallize 18-nm and 39-nm thick room temperature deposited gold thin films on a quartz substrate. Comparison of laser wavelengths confirms that improvements in electrical conductivity up to 40% are achievable for 18-nm gold film when treated with the 515-nm laser, and the 343-nm laser was found to be more effective in crystallizing 39-nm gold films with 29% improvement in the crystallinity. A two-temperature model provides an insight into ultrashort laser interactions with gold thin films and predicts that applied fluence was insufficient to cause melting of gold films. The simulation results suggest that non-equilibrium energy transfer between electrons and lattice leads to a solid-state and melt-free crystallization process. The proposed low fluence femtosecond laser processing method offers a possible solution for a melt-free thin film crystallization for wide industrial applications.