The human body has difficulty repairing damaged dental enamel, an acellular hard tissue. Researchers have sought feasible biomimicry strategies to repair enamel defects; however, few have been successfully translated to clinical applications. In this study, we propose a new method for achieving rapid enamel mineralization under a near-physiological environment. Through treatment with a laser and chelating agents, 15 μm crystals could be grown compactly on an enamel substrate in less than 20 min. The compact crystal layer had similar structure as native enamel prisms and high elastic modulus. This layer also had the potential for further remineralization in saliva. The benefit of using laser can not only speed up the mineralization, but also control the crystal growth precisely where in need. A mechanism for how laser and chelating agents synergistically function is also proposed. This strategy offers a possibility for enamel-biomimicking repair in dental clinics.