Strained epitaxial growth provides the opportunity to understand the dependence of intrinsic and extrinsic properties of functional materials at frozen intermediate stages of a phase transformation. In this study, a combination of thin film experiments and firstprinciples calculations yields the binding energy and magnetic properties of tetragonal Fe 70 Pd 30-x Cu x ferromagnetic shape memory thin films with x = 0, 3, 7 and structures ranging from bcc to beyond fcc (1.07 < c/a bct < 1.57).We find that Cu enhances the quality of epitaxial growth, while spontaneous polarisation and Curie temperature are only moderately lowered as expected from our calculations. Beyond c/a bct > 1.41 the samples undergo structural relaxations through adaptive nanotwinning. For all tetragonal structures, we observe a significant increase of the magnetocrystalline anisotropy constant K 1 , which reaches a maximum of K 1 ≈ -2.4*10 5 Jm -3 at room temperature around c/a bct = 1.33 and is thus even larger than for binary Fe 70 Pd 30 and the prototype Ni-Mn-Ga magnetic shape memory system. Since K 1 represents the driving force for variant reorientation in magnetic shape memory systems, we conclude that Fe-Pd-Cu alloys offer a promising route towards microactuators applications with significantly improved work output. Contents 1. Introduction 2. Experimental and theoretical methods 3. Structure and epitaxial relationship 4. Remanence, coercivity and saturation field 5. Change of Curie temperature and spontaneous polarisation 6. Change of magnetocrystalline anisotropy energy 7. Conclusions Acknowledgments References 1. Introduction Due to huge strains up to 10% [1] magnetic shape memory (MSM) alloys are of particular interest for microactuators [2]. Most research on bulk and thin films focuses on the Ni-Mn-Ga prototype system [3], but in particular for microsystems Fe 70 Pd 30 as the second system discovered [4] shows several advantages. While in the Ni-Mn-Ga system oxidation can result in functional degradation [5] the high content of the noble element Pd in Fe-Pd makes this MSM alloy even biocompatible [6]. Spontaneous magnetic polarisation J S and Curie temperature T C are considerably higher [7,8] compared to Ni-Mn-Ga. Whereas the high material cost hinder bulk applications of Fe-Pd, microsystems require only small masses of active material, which makes the material costs negligible compared to the increased process costs of film preparation.In this paper we quantify the influence of Cu alloying on the magnetic properties of Fe 70 Pd 30-x Cu x . Recent combinatorial experiments revealed that Cu can substantially increase the martensitic transformation temperature [9] which marks the upper limit of the working range for MSM applications. After a thorough crystallographic characterisation of the films we will focus on magnetic aspects, in particular on the magnetocrystalline anisotropy energy.As an intrinsic material property, the anisotropy constant K represents the maximum energy density which can be supplied by an external magnetic fi...