If you want to calibrate a set you will most likely have to go into the service menu and one should really leave that to an isf calibrator with the proper equipment. Or if you dare venture on this route on your own, make sure you write down every value of every line because there is no reset in this menu.
If you want to set-up (I personally can't call it calibration without colour meters and other fancy equipment)your tv with the the options available to you (and on the Samsung it is actually pretty extensive, I know as I own one), I would recommend http://www.lagom.nl/lcd-test/. I ran this to my set through my ps3 and feel this site has given me the best results over any other method I have tried (calibration discs and such). All done by eye so I'm sure it's far from the 6500k standard, but I got it to look as best as my 34 year old eyes can see.
I wonder about using the above images meant to set up a monitor to set up a TV rather than using images specifically designed to set up a TV.
Perhaps someone with a background in this can lend an opinion?
Why not try the simple solution first and get yourself a DVE (digital video essentials) disc for a few bucks and calibrate with that before messing with service menus, especially if you're not experienced with it.
The DVE also has a nice tutorial that explains why you want to have the LCD set properly with the same values a CRT has instead of torch mode and overly bright colours and backlighting the way most sets come shipped from the factory. We had ours blazing until we set them up properly, it takes a couple of days to adjust to the look but when ever I see someones LCD in their home now I cringe.
I use the THX Optimizer found on many DVDs, for example most Pixar titles like Finding Nemo. Samsung's allow you to set different calibrations for each input, so you might have to repeat the calibration for each. Samsung also has three modes, movie, standard and dynamic. I've set those for different lighting conditions or source material, for example, dynamic for video games or bright daylight, standard for computer work and movie for movies and low light. I really don't believe one setting can accomodate all source material.
You'll find the free and simple solutions will meet all your needs.