We discuss our progress in the use of multiple laser beams and multiple targets for the pulsed laser deposition of thin films for waveguide laser and magneto-optic applications. In contrast to the more widely used single-beam/single-target geometries, having more than one laser-produced plume can allow tuning of the material properties and complex engineering of the deposited thin films. For optical applications—the majority of the work reported here—dopants can be selectively introduced, lattice mismatch and residual strain can be compensated, which is an important factor for successful growth of thin films of ∼ tens of microns thickness, and refractive index values can be adjusted for fabrication of sophisticated waveguiding structures. We discuss mixed, layered, superlattice and Bragg reflector growth, which involve out-of-plane engineering of the film structure, and in-plane engineered geometries for designs relevant to thin-film disc lasing devices. Finally we briefly discuss our most recent use of multi-plume growth for magneto-optic thin films, which involves compositional tuning of final magnetic properties.