A low-temperature (90 °C) and directly grown anatase titanium dioxide (TiO2) nanocrystalline film using successive ionic layer adsorption and reaction (SILAR) for perovskite solar cell and gas sensor applications. TiO2 nanocrystalline electron transfer layer (ETL) improves the power conversion efficiency (PCE) of perovskite solar cells due to faster charge transport kinetics as well as slower charge recombination process. The optimized TiO2 nanocrystalline ETL (15 L) demonstrates as high as ~10% PCE with a short circuit current density of 18.0 mA/cm2, open circuit voltage of 0.81 V and fill factor of 66.3% in perovskite solar cells. Furthermore, room-temperature ammonia sensing characteristics of TiO2 nanocrystalline film (25 L) were demonstrated for various concentration levels of ammonia in dry air conditions. A high room-temperature response of 80% was achieved at 100 ppm of ammonia with rapid response and recovery signatures of 30 and 85 s, and nearly fifteen days stability, respectively. The response of the sensor to other gases such as formaldehyde, petrol, ethanol acetone, and ammonia etc, indicated a high selectivity towards volatile organic compounds of ammonia gas. The room temperature operation, with high selectivity, repeatability and fast transition times, suggests potentially useful in flexible and cost-effective production in optoelectrochemical device technology.