There isn’t one magic setting that will allow you to print sharp images at that size. What’s required is a combination of resolution, sharpness, low noise and lack of blur in the image. Don’t get too hung up on the DPI; large images are meant to be viewed from a distance, and don’t need to be printed at the 300 DPI that a smaller image would need to. 108 DPI will be fine for an image meant to be hung on a wall.
Resolution is a good thing to have; the more pixels available to you, the more you can crop your image as you see fit and still have enough resolution to print decent sizes. However, all the resolution in the world will not produce a decent print if the image is misfocussed or lacks sharpness. Unfortunately, some of this sharpness is due to the lens used (in general, more money = better lens) and has nothing to do with the camera settings. Aperture also has an effect on sharpness (more precisely, on depth of field), and for a portrait, you typically want to shoot with a large aperture (small f-number) to isolate your subject from the background. For a landscape where you want as much of the image to be in focus as possible, a small aperture (large f-number) is indicated.
Large aperture used for a portrait (f/2.8): http://anuruddha.smugmug.com/People/Portraits/1256848_Af7Sx#100442228_qmLoi-A-LB
Small aperture used for a landscape (f/10): http://anuruddha.smugmug.com/People/Jersey-2008/Jersey-2008-169/362368089_vo32v-L.jpg
You also need to consider the type of photograph you are taking, to avoid or perhaps create blur for effect. If you want a sharp, frozen in time capture, you need to make sure that your shutter speed is high enough to capture the event. Ideally, the camera should be supported by a tripod to help avoid hand shake. Alternatively, you might want a long exposure for artistic effect, in which case you will almost definitely want a tripod.
Long exposure on a tripod (1/6 s): http://anuruddha.smugmug.com/Street-Scenes/London-Through-a-50/2301793_i48is#120318652_iLX7i-A-LB
Short exposure to freeze runners (1/640 s): http://anuruddha.smugmug.com/People/London-Run-October-2006/IMG7510/100900398_Efbj4-L.jpg
Shooting at the lowest possible ISO will reduce the noise in the image, and improve detail in the print. Artistic “film grain” can always be added later if required. There’s a constant interplay between ISO, aperture and shutter speed that you need to balance to get the right exposure. You want to keep ISO low to avoid noise, but a noisy sharp image is better than a clean blurred one, so if you can’t get a decent shutter speed, you need to up the ISO or open up the aperture. The latter means that you might lose sharpness due to the characteristics of the lens so you might decide that you need a flash…
As you can see, it can be a complex affair! The on-camera settings that I most often change are aperture, ISO and white balance, in that order. I tend to shoot in aperture-priority mode, where I set the aperture and the camera automatically adjusts the shutter speed. If the shutter speed is too low, I open up the aperture a bit or bump the ISO a step higher. I think playing around with these settings will give you a good handle on how to generate sharp images that will print well at large sizes, to be admired by all while hanging on your walls. This turned out much longer than I expected; I hope it’s useful!