Compound crystallization is typically achieved from supersaturated solutions over time, through melting, or via sublimation. Here a new method to generate a single crystal of thioglucoside using a sub-10-fs pulse laser is presented. By focusing the laser pulse on a solution in a glass cell, a single crystal is deposited at the edge of the ceiling of the glass cell. This finding contrasts other non-photochemical laser-induced nucleation studies, which report that the nucleation sites are in the solution or at the air-solution interface, implying the present crystallization mechanism is different. Irradiation with the sub-10-fs laser pulse does not heat the solution but excites coherent molecular vibrations that evaporate the solution. Then, the evaporated solution is thought to be deposited on the glass wall. This method can form crystals even from unsaturated solutions, and the formed crystal does not include any solvent, allowing the formation of a pure crystal suitable for structural analysis, even from a minute amount of sample solution.