This paper proposes a two-degree-of-freedom adaptive output feedback control system design scheme with an adaptive output predictive feedforward for multiple-input-multiple-output (MIMO) LTI systems. In the proposed method, we first present a novel simple adaptive output estimator design scheme by introducing a parallel feedforward compensator. On the basis of the designed adaptive output estimator, the output predictor will be realized and then output predictive controller is designed for feedorwared control. The stability of the proposed method will be maintained by combining ASPR (almost strictly positive real) based output feedback, that is, by designing a two-degree-of-freedom control system. We validate the effectiveness of the proposed adaptive control through experiments on control of a three-tank process.