The theoretical basis for the nuclear cross-section adjustment in the 2-D method of characteristics (MOC) and 1-D SN coupling sensitivity and uncertainty analysis code KYADJ is developed. The energy-dependent sensitivity coefficients are produced by the sensitivity analysis using the 3-D fine flux and adjoint flux based on the first-order perturbation theory. Not only can the sensitivity coefficients be used to estimate the uncertainty of the effective multiplication factor caused by the measurement uncertainties of nuclear cross-section data, but also they can be implemented in the cross-section adjustment according to the Bayes’ theorem and the generalized linear-least-squares method (GLLSM). The cross-section adjustment aims to promote nuclear data evaluations, code verifications, and data validations. In this paper, the adjustment method is verified by the light water reactor (LWR) benchmarks: the MOX pin-cell and the PB-2 assembly cases from the UAM benchmarks. The virtual experimental value is assumed to be the target value of the cross-section adjustment. The results show that the GLLSM can reduce the differences between the calculated and experimental (C/E) values remarkably. All the relative variations of cross-sections for the adjustment are given according to the information of the (C/E) value, the sensitivity coefficients, and the prior uncertainties. The posteriori uncertainties are given, which demonstrates the decrease of the uncertainties.