Printable organic semiconducting single crystals (OSSCs) offer tantalizing opportunities for next-generation wearable electronics, but their development has been plagued by a long-standing yet inherent problem—spatially uncontrolled and stochastic nucleation events, which usually causes the formation of polycrystalline films and hence limited performance. Here, we report a convenient approach to precisely manipulate the elusive molecule nucleation process for one-step inkjet printing of OSSCs with record-high mobility. By engineering curvature of contact line with a teardrop-shaped micropattern, molecule nucleation is elegantly anchored at the vertex of the topological structure, enabling formation of a single nucleus for the subsequent growth of OSSC. Using this approach, we achieve patterned growth of 2,7-dioctyl[1]benzothieno[3,2-b][1] benzothiophene single crystals, yielding a breakthrough for organic field-effect transistor array with high average mobility of 12.5 cm2 V-1 s-1. These findings not only provide keen insights into controlling molecule nucleation kinetics, but also offer unprecedented opportunities for high-performance printed electronics.