The adjustment of laser tracker network measurements for large-scale metrology applications has unique considerations not commonly encountered in the network adjustment approaches generally used in either standard metrology or in traditional geodetic surveying. Many applications that require the measurement accuracy of a laser tracker are confined to small working areas to measure the dimensional quality of manufactured parts. Large-scale metrology applications require the same high measurement accuracy, but over a comparatively larger working area. This paper describes a unified least-squares approach to adjust three-dimensional survey network measurements that takes into account the unique considerations of large-scale metrology networks. The impetus for these unique considerations arises from an application that falls neatly between the disciplines of metrology and geodesy—resembling a mixture of the conditions and requirements from both. This paper will also describe a case study of a large-scale metrology survey network used to align the particle accelerator at Michigan State University’s Facility for Rare Isotope Beams (FRIB).