The development of quantum information technology demands precise engineering and control of quantum states at the single-atom level. Recent advances in electron spin resonance combined scanning tunneling microscopy (ESR-STM) have enabled quantum coherent control of individual atomic and molecular spins on surfaces, marking a significant advance in quantum nanoscience and technology. This review summarized the latest developments in electrically coherent manipulation of surface-based quantum systems, focusing on single atomic and molecular spin manipulation, and multi-spin system dynamics. Special attention is given to recent achievements in universal coherent control, dynamical decoupling and realization of multi-qubit gates, demonstrating the growing potential of surface spin systems as a platform for quantum information processing.