The observation of reflection high energy electron diffraction (RHEED) oscillations has been proved to be a key to open the nano-world of materials, since it definitely verifies that the film growth proceeds in layer-by-layer mode with each layer thickness controllable by simply counting the number of oscillations. This enabled the fabrication of nano-engineered hetero-junctions and devices as commonly practiced for conventional semiconductors and metals. Here we report on the first observation of clear RHEED intensity oscillation in thin film fabrication of a φ-conjugated molecular solid. The observation has been achieved by coupling a novel deposition method using a continuous-wave infrared laser for evaporation and a high sensitive RHEED detector, in addition to the combinatorial optimization of film deposition parameters that facilitated our preceding first success in the layer-by-layer growth of oxide thin films. Some details of system design and experimental conditions are presented to discuss the key factors for atomically controlled film growth of molecular solids.