It could be argued that the square is the 'nicest' rhombus, but the rhombus with angles of 60 and 120 degrees seems nicer still. One of the nice things about the 60/120 rhomb are the plane tilings that can be constructed from it. One of these tilings is the 'tumbling blocks' tiling shown at the top of the post, in which at some points you see 'cubes' (around the degree 3 vertices), while at others you see 'flowers' (around the degree 6 vertices). Because of the two different types of vertices, this is known as a quasi-regular rhombic tiling. (Another tiling that uses the 60/120 rhomb is this one.)
If you want to build a polyhedron that resembles the tumbling block tiling, one method is to reduce the number of petals in your flowers to 5, and then stretch your 60/120 rhombs until they are have angles of 63.435 and 116.565 degrees. Thirty of these rhombs arranged around vertices of degree 3 and 5 produces a quasi-regular polygon known as the rhombic triacontahedron.
The image above is of a model that was built using rhombic units printed onto card stock. (A printable file is here).
Despite the apparent ugliness of the 63.435 and 116.565 degree angle-measurements, our nice 60/120 rhomb has been, arguably, stretched into an even nicer one - a 'golden rhombus,' so called because the ratio of the diagonals is equal to the golden ratio.
The dual of the rhombic triacontahedron is the archemedian polyhedron known as the icosidodecahedron. The image below is of a somewhat decorated model that was built using the units described here.