The directed self assembly of a 3‐miktoarm star terpolymer (polyisoprene‐arm‐polystyrene‐arm‐polyferrocenylethylmethylsilane (3μ‐ISF)) into a (4.82) square symmetry Archimedean tiling pattern is described. Bulk samples of 3μ‐ISF generate equilibrium columnar (4.82) tile patterns (symmetry p 4 mm) on annealing, which is preceded by a metastable c 2 mm centered rectangular structure. In contrast, in thin films of 3μ‐ISF blended with PS homopolymer, the c 2 mm phase is stable with columns oriented out of plane when the film thickness is below 50 nm. However, the 3μ‐ISF/homopolymer blend rapidly forms a p 4 mm symmetry when the film thickness is ∼80 nm, with grain sizes of several μm and excellent order. Defects in the p4mm structure are described. 3‐miktoarm star terpolymer chains consisting of polyisoprene (PI), polystyrene (PS), and polyferrocenylethylmethylsilane (PFS) self‐assemble into a (4.82) Archimedean tiling pattern with PFS (approximately square) domains occupying positions between the approximately octagonal PS and PI.