Open them in an image editing program like Photoshop or GIMP and adjust the overall image size to make it smaller. You may need a specific plugin for either program to do so.
Alternatively, use VTFEdit to export the .VTF as a .TGA file, do the same thing I mentioned previously, then re-import it into VTFEdit to save it as a .VTF file.
If you really want to get the filesize low you can save it in the l8 compression format on import.
There's a couple of ways. The first way is to make sure you aren't importing all of your textures with alpha masks unless it's needed. Importing the texture as a BMP instead of a TGA if the alpha mask is unused with a format that doesn't force an alpha mask will cut the file size in half.
The second is to ensure you're compressing textures. Using the DXT1 format on import will compress them while using something such as RGB888 will not compress them. Some people try to avoid compression for better textures but that just kills file sizes.
Lastly, you can use bzip2 depending on usage. The bz2 format is a compression format supported by Source by default. This can and should be used on files that aren't going to be in the gma format and on the workshop. If it is going on the workshop as a gma file though ignore bzip2 as compression is handled automatically.
You can also use Paint.NET with .vtf plugin and choose 'compressed texture' template when you save your texture.
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