The SCS-CN method is a globally known procedure used primarily for direct-runoff estimates. It also is integrated in many modelling applications. However, the method was developed in specific geographical conditions, often making its universal applicability problematic. This study aims to determine appropriate values of initial abstraction coefficients λ and curve numbers (CNs), based on measured data in five experimental catchments in the Czech Republic, well representing the physiographic conditions in Central Europe, to improve direct-runoff estimates. Captured rainfall-runoff events were split into calibration and validation datasets. The calibration dataset was analysed by applying three approaches: (1) Modifying λ, both discrete and interpolated, using the tabulated CN values; (2) event analysis based on accumulated rainfall depth at the moment runoff starts to form; and (3) model fitting, an iterative procedure, to search for a pair of λ, S (CN, respectively). To assess individual rainfall characteristics’ possible influence, a principal component analysis and cluster analysis were conducted. The results indicate that the CN method in its traditional arrangement is not very applicable in the five experimental catchments and demands corresponding modifications to determine λ and CN (or S, respectively). Both λ and CN should be viewed as flexible, catchment-dependent (regional) parameters, rather than fixed values. The acquired findings show the need for a systematic yet site-specific revision of the traditional CN method, which may help to improve the accuracy of CN-based rainfall-runoff modelling.