The burr removal and finishing of drilled hole walls typically require multiple post-processing steps. This experimental study introduces a novel single-step drilling approach using modified drill bits for simultaneous burr removal and surface finishing in aluminum 6061-T6. The odified-1 drill, equipped with a deburring micro-insert, achieved superior results, with a chamfer height of −2.829 mm, drilling temperature of 40.28 ◦C, and surface roughness of 0.082 µm under optimal conditions. Multi-objective optimization using the RSM and MOGA-ANN identified the optimal drilling parameters for the Modified-1 drill at 3000 rpm under water lubrication as compared to dry conditions and kerosene. Experimental validation confirmed the high prediction accuracy, with deviations under 6%. These results establish the Modified-1 twist drill bit with a deburring micro-insert as a highly effective tool for burr-free high-quality drilling in a single operation. This innovative drill design presents an efficient, single-step solution for burr elimination, chamfer formation, and surface finishing in drilling operations.