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An electroless phosphorus nickel-carbon nanotube (Ni-P-CNT) nanocomposite film synthesis and related process for microelectromechanical systems device fabrication have been successfully developed and presented in this paper. With a special acid oxidative method, a well-dispersed nickel-CNT's colloidal solution has been produced without any aggregation, which is very suitable for microstructure fabrication. The nanoindentation measurement indicates that the Young's modulus and hardness of the Ni-P-CNT's nanocomposite film plated in the bath with 0.028-g/L CNTs can greatly increase up to 665.9 and 28.9 GPa, respectively, which are approximately four times larger than that of pure nickel. Moreover, the content of CNTs in the Ni-P-CNT's films is measured by an elemental analyzer. Via the electrical resistivity measurement using a four-point probe, it is found that the electrical property of the nanocomposite film can be well characterized using a Maxwell-Wagner model for a two-phase mixture. The performance improvements of the electrothermal microactuator made of the nanocomposite, including device strength and power efficiency, have been proven similar to the actuator made of the Ni-diamond composites by electrolytic plating by Tsai et al., but with more efficiency and higher strength than the Ni-diamond device does.