Controlled doping of carbon nanotubes is elemental for their electronic applications. Here we report an approach to tune the polarity and degree of doping of single-walled carbon nanotubes via filling with nickelocene followed by encapsulated reactions. Using Raman, photoemission spectroscopy and transmission electron microscopy, we show that nickelocene molecules transform into nickel carbides, nickel and inner carbon nanotubes with reaction temperatures as low as 250 °C. The doping efficiency is determined for each chemical component. Synchronous charge transfer among the molecular components allows bipolar doping of the carbon nanotubes to be achieved in a broad range of ±0.0012 e− per carbon.