Neodymium titanate ((Formula presented.)) is a ferroelectric as well as a pyroelectric material with a transition temperature of 1480 °C. Hence, (Formula presented.) offers potential to be utilized as high temperature pyroelectric sensor in both bulk and thin film form. In this work, bulk (Formula presented.) powders were synthesized using solid state reaction method, which were later pressed into the pellets. Later, thin films of (Formula presented.) were deposited on commercially available platinized(111) silicon and Si(100) substrates via pulsed laser deposition technique. The huge c/a ratio (∼1.695) and the thermal expansion mismatch with most of the commonly used substrates like silicon and platinized silicon, results into crack formation in (Formula presented.) thin films. Crack formation on (Formula presented.) thin film, which deteriorates pyroelectric property of (Formula presented.) film, was suppressed by the introduction of (Formula presented.) buffer layer between the film and substrate. The calculated value of thermal expansion coefficient of (Formula presented.) is 2.86 × 10−5 °C−1. Moreover, thermally generated strain between (Formula presented.) film and platinum substrate was found to be around 2%. The piezoresponse force microscopy experiment confirms the existence of ferroelectric domains in the film. Pyroelectric coefficient (p) calculated from the pyrocurrent studies was estimated around 3.52 and 13.6 μC/m2K in the bulk and thin film, respectively. © 2022 Taylor & Francis Group, LLC.