You're probably going to want to use Bitlocker with your smart card. This will effectively encrypt your drive/files so that they are only accesible via your smart card. This is a good strategy to use if you have a backup of your smart card in the event that it's lost or destroyed.
Using Smart Cards with BitLocker
http://www.windowsecurity.com/articles/Best-practice-guide-how-configure-BitLocker-Part1.html
Warning
Note: In order to use Bitlocker to encrypt your home system you will need to upgrade to Windows 7 Ultimate or Enterprise, as all other versions do not come with Bitlocker. You could always use a different authentication method
TrueCrypt is an open source security program which allows you to encrypt your entire hard drive or specific file sets. You can require a password and/or a key file in order to log in. This could feasibly be done with a smart card I believe.
http://www.truecrypt.org
http://www.truecrypt.org/docs/?s=keyfiles
Tip
My advice would be to use
TrueCrypt to encrypt a particular portion of your hard drive in which you store all of your sensitive files. This would allow you to log into your computer without enhanced security yet you wouldn't be able to access your secure files without a different password and keyfile. You can enhance this security with
KeePass, an open source password storage utility which can store encrypted passwords. This type of software enables you to use extremely long and complicated passwords without the need to remember them. Whenever you need to log into a website you just open you keepass software via a password and keyfile.
Either way, you can encrypt either a portion or your entire hard drive using TrueCrypt and then encrypt your passwords using KeePass. This would allow you to keep your computer safe from predators, and furthermore keep your passwords even safer.
An example of the difference KeePass makes other than the fact that your passwords are stored securely can be seen below.
Password without KeePass: My19PasSW0rD
This is easy to remember so that you don't have to store it in a password database, however it's also low on security due to the fact that a long password is hard to remember
Password with KeePass: Ë÷J$;Án#„ÅÝ ºôzªŽT9KºbhœK‘ZJ¥R¬p×$Á°µoúñƒ§™?gãÏ£ÝerV¡6ˆûÁtïôäj
There are two versions of KeePass, one that you can store on a flash drive and take with you anywhere and use on any computer. This allows you to have these long complicated passwords and use them on any computer.
The other version is that which you install on a computer. TrueCrypt has the same portability, but isn't used as frequently useless you wish to encrypt usb drives.