Epitaxial growth of triangular CdS nanoplates by dip-pen nanolithography is achieved on a mica substrate. This method offers in situ initiating, controlling, and monitoring of the epitaxial growth of triangular CdS plates in nanoscale. Control experiments and structure analysis indicate that both the tip-modulated crystallization and matching in the crystal structures (symmetry and lattice) of CdS and mica play key roles in the epitaxial growth of well-crystallized CdS nanostructures.