The spectrum sensing that jointly estimates direction-of-arrival (DOA) and frequency spectrum is an important issue for cognitive radio. Existing off-grid DOA estimation algorithms using difference coarray require a large number of snapshots to guarantee the estimation accuracy. Meanwhile, inaccurate DOA estimation renders inaccurate frequency spectrum estimation due to coupled estimation process. In order to overcome these disadvantages, we propose a joint angle and frequency spectrum estimation algorithm using difference coarray in this work. The proposed algorithm first transforms the received signal into the coarray domain and then adopts an “estimate and subtract” method to separate multiple signals. Subsequently, the DOA estimate of each source is corrected iteratively based on the proposed simple interpolation method. Finally, the frequency spectra are obtained by estimating the frequency response matrix based on the previous estimated DOAs. The shortage of requiring a large number of snapshots are overcome by utilizing the deterministically orthogonal signal model in which the signals are completely uncorrelated. Simulation results demonstrate the effectiveness of the proposed algorithm for off-grid DOA and frequency spectrum estimation using difference coarray with few snapshots.