Current perception systems often carry multimodal imagers and sensors such as 2D cameras and 3D LiDAR sensors. To fuse and utilize the data for downstream perception tasks, robust and accurate calibration of the multimodal sensor data is essential. We propose a novel deep learning-driven technique (CalibDNN) for accurate calibration among multimodal sensor, specifically LiDAR-Camera pairs. The key innovation of the proposed work is that it does not require any specific calibration targets or hardware assistants, and the entire processing is fully automatic with a single model and single iteration. Results comparison among different methods and extensive experiments on different datasets demonstrates the state-of-the-art performance.