Despite the high economic and safety impact of food adulteration, food surveillance is limited by high costs and limited resources available to regulatory agencies. Infrared (IR) spectroscopy can provide rapid and cost-effective tools for effective food surveillance and deter acts of economic adulteration, counterfeiting, or vandalism. Powerful pattern recognition techniques can be used to screen materials and enable real-time and field-based measurements for controlling the raw material stream. This chapter presents the current state of research on applications of IR for authentication of high-value raw materials susceptible to economically motivated tampering. In addition, we present Raman spectroscopy as a complementary vibrational technique with increasing relevance to the surveillance of ingredient authenticity. We will review sensor technologies directed at improving efficiency, throughput, and reliability, presenting examples of recent cases of adulteration that resulted in high costs to the food industry. Finally, portable devices are introduced as the future of IR for field applications.