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Is your PC more than capable of running your emulator of choice? Can you run it with 4-8x AA and 4-8x AF (and the next increase is not visually worth the resources used) or higher or even maxed out? Many emulators will let you increase the internal resolution of the game textures, and apply texture filters, such as 2xSAL or HQ4X. There are even ways to add in more post-processing shaders, like cell-shading, Bloom + HDR, Blur, Sharpen, etc., but those are personal preference, and a good portion of people believe they usually make the game look worse.
What we can do if use some external programs to further increase the graphical quality of these emulators (they are 'made' for PC games, but they can work on most emulators also) and they can be fairly easily configured to customize how you want your games to look. I do not have a lot of experience with these 2 programs, so I will not be posting instructions on how to setup/use/configure them; but for those who may not have heard of these, I will be linking the programs. Note: users of MSI Afterburner who use it to monitor DirectX statistics such as FrameRate, may need to open up the RTSS (MSI On-Screen Display) and in settings check 'Enable compatibility with modified Direct3D runtimes libraries' or your program may fail to launch while MSI AB is running.

1. ENB Series. Developed by Boris Vorontsov, this can be either injected (in some cases this is not possible and will lead to the program not launching, then you will have to use the second method) or by placing the modified d3d9.dll file in the .exe's folder. This can be used for any program that utilizes DirectX 9. Games that support DirectX 9 or 10/11 with proper hardware will default back to DX9.

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http://www.enbdev.com/index_en.htm

2. SweetFX. This program will work with any DirectX 9, 10, or 11 game if your Graphics Processor supports at least Shader Model 3. It currently is supported for 32-bit programs, but there is a Work In Progress download you can try on the main page for 64-bit programs.

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http://forums.guru3d.com/showthread.php?t=376265

There is also a configurator for this program, which will make it more simple to change some settings. It can be found at:

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http://sweetfx.thelazy.net/?p=91

Here are some personal screenshots showing Final Fantasy X with PCSX2 before, middle, and after.
All shots are ran from plugin GSdx 5627 SSE4.1 v0.1.16 @1920x1080 Direct3D11.
Before is ran with no enhancements with the default PS2 Internal Resolution. The middle and end increased the Internal Resolution to 1260x709 with 8xMSAA and texture filtering on. The end added a basic SweetFX preset I threw on for the screenshot for better lighting and color saturation (still at 1260x709 + 8xMSAA @1920x1080).

I have never used these but I might now. Thanks for a great topic that was well illustrated.

Generally I just use the Hardware acceleration that comes built in to the emulators and my PCSX 2 looks amazing, almost better than that in 1080p... I haven't ever needed an external program to make it look better... but what the heck. I might give this a go later on.