This dissertation develops new approaches for detection and classification of buried radioactive materials. Different spectral transformation methods are proposed to effectively suppress noise and to better distinguish signal features in the transformed space. The contributions of this dissertation are detailed as follows. 1) Propose an unsupervised method for buried radioactive material detection. In the experiments, the original Reed-Xiaoli (RX) algorithm performs similarly as the gross count (GC) method; however, the constrained energy minimization (CEM) method performs better if using feature vectors selected from the RX output. Thus, an unsupervised method is developed by combining the RX and CEM methods, which can efficiently suppress the background noise when applied to the dimensionality-reduced data from principle component analysis (PCA). 2) Propose an approach for buried target detection and classification, which applies spectral transformation followed by noisejusted PCA (NAPCA). To meet the requirement of practical survey mapping, we focus on the circumstance when sensor dwell time is very short. The results show that spectral transformation can alleviate the effects from spectral noisy variation and background clutters, while NAPCA, a better choice than PCA, can extract key features for the following detection and classification. 3) Propose a particle swarm optimization (PSO)-based system to automatically determine the optimal partition for spectral transformation. Two PSOs are incorporated in the system with the outer one being responsible for selecting the optimal number of bins and the inner one for optimal bin-widths. The experimental results demonstrate that using variable bin-widths is better than a fixed bin-width, and PSO can provide better results than the traditional Powell’s method. 4) Develop parallel implementation schemes for the PSO-based spectral partition algorithm. Both cluster and graphics processing units (GPU) implementation are designed. The computational burden of serial version has been greatly reduced. The experimental results also show that GPU algorithm has similar speedup as cluster-based algorithm.