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This paper presents a cross-covariance-based time- delay estimation method for accurate determination of the time- delay between the input and the output of a RF power amplifier/transmitter. In order to overcome the time resolution limitation caused by the relative low sampling rate of the analog- to-digital converter in the baseband signal acquisition system, the Lagrange interpolation is utilized to improve the time resolution. A two-step method for time-delay estimation/alignment is proposed to increase the dynamic range for time-delay estimation/alignment under the certain computation resource consumption condition. The experimental validation results have been provided to illustrate the effectiveness of the proposed approach for accurate time-delay estimation and alignment.