Strong green and red visible emissions were obtained from ZrO2:Yb3+–Er3+ nanocrystals synthesized by sol-gel method and annealed at 1000 °C for 5 h. The average crystallite size was ∼70 nm with tetragonal phase for total concentration lower than 3 mol % and cubic phase for concentration higher than 5 mol %. The color coordinate of the upconverted signal was tailored by controlling the dopant composition that change the red/green ratio dominated by the cross relaxation and energy back transfer process as was demonstrated theoretically and confirmed experimentally. Both coefficients were calculated, C51∼1.02×10-16 and C5b∼6.04×10-17, from the theoretical model based on the rate equations. The highest energy transfer efficiency was η∼64% for 2 mol % of Yb and 2 mol % of Er3+. However, for the highest upconverted signal was only η∼29% obtained for 2 mol % Yb and 1 mol % Er with effective decay time τeff∼438 μs for red and τeff∼290 μs for green band.