Components with super-smooth freeform surfaces are being applied more and more extensively in various fields. Among the valuable non-traditional finishing processes for generating super-smooth freeform surfaces that have been developed, the two-axis vibration assisted polishing process has attracted great attention from some scholars in recent years. However, in the existing two-axis vibration assisted polishing process, vibrational coupling occurs between the traverse and axial directions in the vibrating body and causes the actuating polishing tool to rotate, which limits the polishing effect. To solve the above-mentioned vibration coupling problem, herein we develop a novel two-dimensional ultrasonically actuated polishing process using two mutually perpendicular Lange in vibrators. Through theoretical analysis and experimental tests, the influences of the contact pressure, feed rate, and vibrational parameters on the material removal rate of the proposed polishing process were revealed. The experiments demonstrated that the polishing removal rate was greatly improved.