A method for controlling engagement of a power take-off (PTO) clutch of a work vehicle may generally include transmitting, by a computing device, a control signal associated with initiating engagement of the PTO clutch, determining a clutch slippage energy generated during engagement of the PTO clutch due to clutch slippage and, while the PTO clutch is getting engaged, calculating a clutch engagement time remaining until engagement of the PTO clutch is completed based on the clutch slippage energy and a maximum clutch engagement energy associated with the PTO clutch. In addition, the method may include determining a torque command for controlling engagement of the PTO clutch as a function of the remaining clutch engagement time and controlling the engagement of the PTO clutch based on the torque command.