Here we described the synthesis of highly pure double walled carbon nanotube (DWNT) through a right combination of a catalytic chemical vapor deposition method and the two-step purification and evaluated their stacking infidelity when compared to multi-walled carbon nanotubes (MWNTs). Easy fabrication of thin and flexible, but mechanically tough DWNT-buckypaper was due to the long and large-sized bundled DWNT (up to 50 nm), where DWNTs with diameter below 2 nm were packed in hexagonal array. Through detailed transmission electron microscope, X-ray and Raman studies, we confirmed that the intershell spacing of our DWNT sample was ca. 0.36 nm, which was believed to strongly affect negative and small magnetoresistance absolute value of -0.09 at 77 K and 1 T.