Magnetoelectronic multilayer devices are widely used in today's information and sensor technology. Their functionality, however, is limited by the inherent properties of magnetic exchange or dipolar coupling which constrain possible spin configurations to collinear or perpendicular alignments of adjacent layers. Here, a deposition procedure is introduced that allows for a new class of layered materials in which complex spin structures can be accurately designed to result in a multitude of new and precisely adjustable spintronic and magnetoresistive properties. The magnetization direction and coercivity of each individual layer are determined by the deposition process in oblique incidence geometry and can be completely decoupled from neighboring layers. This applies for layers of any ferromagnetic material down to layer thicknesses of a few nm and lateral dimensions of a few 100 nm, enabling the design of efficient and compact magnetoelectronic devices, encompassing precision magnetoresistive sensors as well as layer systems with multiple addressable remanent states for magnetic memory applications.