Enhancing photoluminescence quantum yield and excellent transport associated with molecular order are important for advancing organic laser device performance. However, materials combining excellent quantum yield and transport are rare. 4,4'-Bis[(N-carbazole)styryl]biphenyl (BSB-Cz) has been heavily investigated as a promising material for laser devices. However, research on highly ordered BSB-Cz crystalline films is lacking, despite the much better transport properties to be expected. Here, we show that BSB-Cz thin-film crystals can be prepared using a simple vacuum deposition method, followed by thermal annealing. The resulting crystalline neat BSB-Cz thin films show a very high photoluminescence quantum yield of over 85% and superior optical stability compared to amorphous BSB-Cz films under intense pumping conditions. We believe that our work provides a route for advancing organic laser devices through introducing crystallinity in emitter thin films with a scalable approach.