Pursuing the exotic quantum spin liquid (QSL) state in the Kitaev material α-RuCl3 has intrigued great research interest recently. A fascinating question is on the possible existence of field-induced QSL phase in this compound. Here we perform a high-field measurement of the magnetization process of α-RuCl3 up to 102 T employing the non-destructive and destructive pulsed magnets. Under the out-of-plane field along the c * axis (i.e., perpendicular to the honeycomb plane), two quantum phase transitions are uncovered at respectively 36 T and about 83 T, between which there lies an intermediate phase as the predicted QSL. By measuring the magnetization data with fields tilted from the c * axis up to 90 • (i.e., in-plane direction), we obtain the field-angle phase diagram that contains the zigzag, paramagnetic, and QSL phases. Based on the accurate K-J-Γ-Γ model of α-RuCl3, we perform density matrix renormalization group simulations and reproduce the quantum phase diagram in excellent agreement with experiments.