A Raman probe system includes: a base station; a mobile robot remotely controllable from the base station; a Raman probe assembly supported by the robot, the Raman probe assembly including a laser and a spectrometer; a camera supported by the robot; and a communication subsystem operable to communicate images from the camera and results from the Raman probe assembly to the base station. In some embodiments, a Raman probe system includes: a mobile robot remotely controllable from a base station, the robot including a body and an articulated arm; a camera supported by the robot; a Raman probe assembly supported by the robot, the optical control assembly mounted on the body of the robot; and an optical probe mounted on the articulated arm of the robot; and a wireless communication system operable to communicate images from the camera and results from the Raman probe assembly to the base station.