We investigate the behavior of colloidal particles immersed in a binary liquid mixture of water and 2,6-lutidine in the presence of a chemically patterned substrate. Close to the critical point of the mixture, the particles are subjected to critical Casimir interactions with force components normal and parallel to the surface. Because the strength and sign of these interactions can be tuned by variations in the surface properties and the mixtures temperature, critical Casimir forces allow the formation of highly ordered monolayers but also extend the use of colloids as model systems.PACS numbers: 82.70. Dd, 68.35.Rh, 81.16.Dn Analogous to the geometrical confinement of quantumelectrodynamical (QED) vacuum fluctuations between two parallel metallic plates [1], the constraint of concentration fluctuations in fluid mixtures close to their critical point gives rise to critical Casimir forces acting on the confining surfaces [2]. The range of this interaction is set by the bulk correlation length ξ of the mixture which diverges when approaching the critical point. Therefore, critical Casimir forces are sensitive to minute changes in temperature. Despite several quantitative measurements of such forces [3,4], it was only recently when the amplitude of measured critical Casimir forces in quantumand classical liquids has been directly compared to theoretical predictions [5,6,7,8]. Direct force measurements of a single colloidal particle above a flat surface and immersed in a critical water-lutidine mixture demonstrated, that critical Casimir interactions can easily exceed multiples of the thermal energy k B T [8]. Accordingly, they offer a versatile opportunity to control the pair interaction in colloidal suspensions by weak temperature changes [9,10]. Apart from their exquisite temperature dependence, critical Casimir forces respond sensitively to the chemical properties of the confining surfaces. Depending on whether both surfaces preferentially attract the same mixture's component or not (symmetric or asymmetric boundary conditions), attractive or repulsive critical Casimir forces arise [8,11,12].So far, experimental investigations of critical Casimir interactions were limited to homogeneous surfaces (in contrast to QED Casimir forces [13]) where the corresponding forces act perpendicular to the confining walls. However, when one or both surfaces are chemically patterned, also lateral critical Casimir forces have been predicted [14] In this Letter we experimentally study the interaction between colloidal particles and chemically patterned substrates immersed in a binary critical mixture. Close to the critical point lateral critical Casimir forces lead to the formation of highly ordered colloidal assemblies whose structure is controlled by the underlying chemical pattern. This may suggest a novel route for templated growth of colloidal crystals. At higher particle concentrations, additional critical Casimir forces between nearby particle surfaces arise and eventually lead to the formation of three-dimensional, face...