Recently, a high internal surface of the titanium alloy pipe is required due to the increment of various applications of the pipe such as aerospace. However, the traditional machining process is unable to effectively polish the internal surface of the slender pipe. Thus, a vertical magnetorheological polishing (VMRP) apparatus is carried out in this work to implement high polishing performance on the internal surface of the titanium alloy pipe. The polishing process is realized by the combination of the rotating motion of the pipe and the reciprocating linear motion of the polishing head. Moreover, a series of comparative experiments are conducted to investigate the polishing mechanism of magnetorheological (MR) fluid and enhance the polishing performance. It is shown from the experimental results that proposed VMRP approach exhibits the better polishing performance than the conventional horizontal MR polishing method under same testing conditions. This is because the proposed VMRP method well eliminates the traces of polishing particles owing to the combination of polishing particles with different sizes. In addition, it is identified from the experimental test that the polishing time of the VMRP required to achieve the same polishing effect as the conventional method is shortened under the combination of different rotation speeds. It is identified from the above benefits of the VMRP that the final surface roughness after polishing is below 0.05 μm.