A Cu-Fe-P copper alloy was processed by accumulative roll-bonding (ARB) for ultra grain refinement and high strengthening. Two 1mm thick copper sheets, 30 mm wide and 300 mm long, were first degreased and wire-brushed for sound bonding. The sheets were then stacked on top of each other and roll-bonded by about 50% reduction rolling without lubrication at ambient temperature. The bonded sheet was then cut into two pieces of the same dimensions and the same procedure was repeated for the sheets up to eight cycles. Microstructural evolution of the copper alloy with the number of the ARB cycles was investigated by optical microscopy (OM), transmission electron microscopy(TEM), and electron back scatter diffraction(EBSD). The grain size decreased gradually with the number of ARB cycles, and was reduced to 290 nm after eight cycles. The boundaries above 60% of ultrafine grains formed exhibited high angle boundaries above 15 degrees. In addition, the average misorientation angle of ultrafine grains was 30 degrees.