The structural models of three synthetic Al-substituted goethite specimens have been refined from the neutron data, including crystallographic determinations of the Al levels and H positions. The d-I data were calculated for the final models. A relationship between the c unit cell parameter and Al content has been extended to the entire goethite-diaspore solid-solution system, which makes the regression equation procedure simpler and more accurate. A second prospective H site could not be confirmed because of the quality of existing neutron data. However, it is hoped that a further neutron powder diffraction study of a synthetic, fully deuterated goethite material may allow the existence of the site to be demonstrated.