Microwire microelectrode arrays (MEAs) are implanted in the brain for recording neuron activities to study the brain function. Among various microwire materials, carbon fiber stands out due to its small diameter (5–10 μm), relatively high Young's modulus, and low electrical resistance. Microwire tips in MEAs are often sharpened to reduce the insertion force and prevent the thin microwires from buckling. Currently, carbon fiber MEAs are sharpened by either torch burning, which limits the positions of wire tips to a water bath surface plane, or electrical discharge machining, which is difficult to implement to the nonelectrically conductive carbon fiber with parylene-C insulation. A laser-based carbon fiber sharpening method proposed in this study enables the fabrication of carbon fiber MEAs with sharp tips and custom lengths. Experiments were conducted to study effects of laser input voltage and transverse speed on carbon fiber tip geometry. Results of the tip sharpness and stripped length of the insulation as well as the electrochemical impedance spectroscopy measurement at 1 kHz were evaluated and analyzed. The laser input voltage and traverse speed have demonstrated to be critical for the sharp tip, short stripped length, and low electrical impedance of the carbon fiber electrode for brain recording MEAs. A carbon fiber MEA with custom electrode lengths was fabricated to validate the laser-based approach.