Ultracold single molecules have wide-ranging potential applications, such as ultracold chemistry, precision measurements, quantum simulation, and quantum computation. However, given the difficulty of achieving full control of a complex atom-molecule system, the coherent formation of single molecules remains a challenge. Here, we report an alternative route to coherently bind two atoms into a weakly bound molecule at megahertz levels by coupling atomic spins to their two-body relative motion in a strongly focused laser with inherent polarization gradients. The coherent nature is demonstrated by long-lived atom-molecule Rabi oscillations. We further manipulate the motional levels of the molecules and measure the binding energy precisely. This work opens the door to full control of all degrees of freedom in atom-molecule systems.