The development of new, and the enhancement of existing element-sensitive imaging methods utilizing neutrons of different energy regions was the aim of the European ANCIENT CHARM project. During the present work the setup for Prompt Gamma-ray Activation Analysis (PGAA) at the research reactor FRM 2 in Garching near Munich was modified to enable the spatial mapping of elemental abundances in the analysed samples. Because the PGAA setup at FRM 2 was under construction at the beginning of the project first tests and the development of calibration and measurement procedures for the new imaging method were done by the PGAA group at the Budapest Research Reactor in cooperation with the Institute for Nuclear Physics of the University of Cologne. Due to the higher neutron flux at the PGAA setup at FRM 2 the equipment was transferred from the Budapest Research Reactor to FRM 2 after the PGAA setup at FRM 2 started its regular operation. After further optimizations and the characterization of the setup, measurements were started on replicas of real archaeological objects before several measurements on real objects were performed and analysed. Several measurement configurations were applied. Additional to 2D and 3D imaging measurements a new application for the measurement of thin surface layers in the order of a few 100 micro-meters was developed. For the quantitative analysis of elemental distributions the exact knowledge of the neutron flux at each measured position in the analysed sample has to be known. Based on the well-established cold Neutron Tomography (NT) method a method and software have been developed, which enables the calculation of the neutron flux inside samples with the map of attenuation properties obtained through NT. A new data acquisition system was developed for the regular operation of the PGAA setup at FRM 2, which supports traditional bulk PGAA measurements as well as measurements in the new imaging configuration. The high automation of the system allows a significantly more efficient use of the available measurement time than it was the case before. The new software �HDTV� for the analysis of gamma-ray spectra, which is currently under active development at the Institute for Nuclear Physics of the University of Cologne, was extended by some functionality for the analysis of PGAA spectra. It is a proposed modern successor of the currently used software �TV� and allows the semiautomatic analysis of multiple, similar spectra, what is essential for the new imaging PGA method.