A constrained high-order statistical algorithm is proposed to blindly deconvolute the measured spectral data and estimate the response function of the instruments simultaneously. In this algorithm, no prior-knowledge is necessary except a proper length of the unit-impulse response. This length can be easily set to be the width of the narrowest spectral line by observing the measured data. The feasibility of this method has been demonstrated experimentally by the measured Raman and absorption spectral data.