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In recent years, Vehicle-to-Vehicle (V2V) and Vehicle-to-Infrastructure (V2I) communication brings more and more attention from industry (e.g., Google and Uber) and government (e.g., United States Department of Transportation). These Vehicle-to-Everything (V2X) technologies are widely adopted in future autonomous vehicles. However, security issues have not been fully addressed in V2V and V2I systems, especially in key distribution and key management. The physical layer key generation, which exploits wireless channel reciprocity and randomness to generate secure keys, provides a feasible solution for secure V2V/V2I communication. It is lightweight, flexible, and dynamic. In this paper, the physical layer key generation is brought to the V2I and V2V scenarios. A LoRa-based physical key generation scheme is designed for securing V2V/V2I communications. The communication is based on Long Range (LoRa) protocol, which is able to measure Received Signal Strength Indicator (RSSI) in long-distance as consensus information to generate secure keys. The multi-bit quantization algorithm, with an improved Cascade key agreement protocol, generates secure binary bit keys. The proposed schemes improved the key generation rate, as well as to avoid information leakage during transmission. The proposed physical layer key generation scheme was implemented in a V2V/V2I network system prototype. The extensive experiments in V2I and V2V environments evaluate the efficiency of the proposed key generation scheme. The experiments in real outdoor environments have been conducted. Its key generation rate could exceed 10 bit/s on our V2V/V2I network system prototype and achieve 20 bit/s in some of our experiments. For binary key sequences, all of them pass the suite of statistical tests from National Institute of Standards and Technology (NIST).