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In this paper, a novel high-order optimal terminal iterative learning control (high-order OTILC) is proposed via a data-driven approach for nonlinear discrete-time systems with unknown orders in the input and output. The objective is to track the desired values at the endpoint of the operation cycle. The terminal tracking errors over more than one previous iterations are used to enhance the high-order OTILC's performance with faster convergence. From rigor of the analysis, the monotonic convergence of the terminal tracking error is proved along the iteration direction. More importantly, the condition for a high-order OTILC to outperform the low-order ones is first established by this work. The learning gain is not fixed but iteratively updated by using the input and output (I/O) data, which enhances the flexibility of the proposed controller for modifications and expansions. The proposed method is data-driven in which no explicit models are used except for the input and output data. The applications to a highly nonlinear continuous stirred tank reactor and a highly nonlinear fed-batch fermentater demonstrate the effectiveness of the proposed high-order OTILC design. [ABSTRACT FROM AUTHOR]