Yes, you can.
Maybe in a parallel universe, ie programming a PIC. [would be nice if "just once" there was some
explanation attached to those comments, so we wouldn't have to be mind readers all the time].
I have PICKIT2 and PICKIT3 and actually do most of my programming on PICs. The PICKITs and PICs in
general use completely different programming algorithms from AVR, and have 3 output pins, Mclr/Vpp
[typically 13V for programming], plus SCLK and SDA lines, which are not Sclk, MOSI, MISO.
Also, I've used the UART mode of the PICKIT and it really doesn't work all that well for some reason,but
maybe could be jiggered for downloading sketches to an Arduino bootloader [which is unnecessary in any
case], but doubtful for recoding a raw AVR. Better to use an FTDI Friend/etc on a board without a USB
chip.
I also bought one of the AVR programming dongles from Pololu, but never could get it installed properly on
my notebook, so to burn bootloaders, I use 2 Arduino boards connected via the ICSP headers, and run the
bootloader sketch from the IDE on the master board.