Light-emitting diode (LED) MR16 lamps, regarded as one typical general lighting product of LEDs, are being widely used in many applications. Light efficiency into a main beam and uniformity are two key issues for high quality illumination of LED MR16 lamps. In this study, a practical and precise nonimaging optical design method is presented, and two novel 90- and 120-deg free-form lenses for high illumination quality LED MR16 lamps are designed according to this method. Based on the Monte-Carlo ray-tracing method, numerical simulation results demonstrate that the light output efficiencies of these novel lenses reach as high as 98% and are 17% higher than that of traditional total internal reflection (TIR) MR16 lens. Moreover, more than 89% of light exiting from the surfaces of these novel lenses irradiate within the desired receive target, while only 60% irradiate for traditional TIR lens. The uniformities of illuminance distribution across the target of these novel MR16 lamps also are much higher. In addition, these novel lenses are both quite compact and no more than 1/5 of that of the TIR lens. Therefore, these LED MR16 lamps integrated by novel lenses provide an effective solution to high quality illumination.