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BaLa2ZnO5:Er3+/Yb3+ has been synthesized via a high temperature solid-state method, and the tunable upconversion luminescence and energy transfer process between Yb3+ and Er3+ in this system have been demonstrated. Upon 980 nm laser excitation, the intense green and red emission around 527, 553, and 664 nm were observed for BaLa2ZnO5:Er3+/Yb3+, which can be assigned to the characteristic energy level transitions of 2H11/2 → 4I15/2, 4S3/2 → 4I15/2, and 4F9/2 → 4I15/2 of Er3+, respectively. The critical Er3+ quenching concentration (QC) was determined to be about 5 mol%, and the power studies indicated that mixture of 2- and 3-photon process was responsible for the green and red upconversion luminescence.