Laser ultrasonic testing (LUT) can realize contactless and instantaneous non-destructive testing, but its signal-to-noise ratio must be improved in order to measure carbon fiber reinforced plastics (CFRPs). We have developed a mid-infrared (mid-IR) laser source optimal for generating ultrasonic waves in CFRPs by using a wavelength conversion device based on an optical parametric oscillator. This paper reports a comparison of the ultrasonic generation behavior between the mid-IR laser and the Nd:YAG laser. The mid-IR laser generated a significantly larger ultrasonic amplitude in CFRP laminates than a conventional Nd:YAG laser. In addition, our study revealed that the surface epoxy matrix of CFRPs plays an important role in laser ultrasonic generation.