We demonstrate coherent control of two nuclear spins mediated by the magnetic resonance of a hyperfine-coupled electron spin. This control is used to create a double-nuclear coherence in one of the two electron spin manifolds, starting from an initial thermal state, in direct analogy to the creation of an entangled (Bell) state from an initially pure unentangled state. We identify challenges and potential solutions to obtaining experimental gate fidelities useful for quantum information processing in this type of system. Introduction.-Solid-state spin systems are interesting candidates for quantum information processing: the small systems explored in the lab today are excellent test beds for the ideas of quantum control and quantum error correction, and it may be possible to reach enough qubits for nontrivial quantum computations or to integrate these systems into useful hybrid devices for quantum communications [1] or quantum sensors [2]. The past two decades have seen much progress in the high-fidelity control of small quantum processors realized by nuclear magnetic resonance [3,4], electron spin resonance (ESR) [5][6][7][8][9], and electron-nuclear double resonance [10][11][12][13]. These experiments have served as benchmarks for experimentally attainable gate fidelities [14] and have spurred the development of robust quantum control methods [15,16]. Hybrid electron-nuclear spin systems make it possible to exploit the strengths of each type of spin: electron spin for initialization, readout, and control and nuclear spin for long storage and coherence times [12,13,17]. In particular, it is advantageous to use the electron spin as an actuator to gain full control of the system's spin dynamics via the anisotropic part of the hyperfine interaction [5,18]. Since the hyperfine interaction to nearby nuclei can be of order 1-100 MHz, fast electron-nuclear and nuclear-nuclear gates can be realized by this approach. Several prior studies have demonstrated coherent control of a one electron þ one nuclear spin system using a modulated microwave field in concert with anisotropic coupling [5,7,8]. In this work, we demonstrate an entangling gate between two nuclear spins fully mediated by control of the electron spin. This is an important first step towards achieving efficient control of hybrid electron-nuclear spin systems of interest for quantum information processing.Experiment.-The spin system employed here is based on the stable radical of malonic acid in the solid state [5,7,8,10] with an additional 13 C labeling. X-ray irradiation removes a proton from the methylene group, leaving