1. Weather plays an very important role. If you don't have any fancy payware packages, try using these settings that I use: Click on the "Building Storms" weather theme and click "Ok" Then go back to the weather options, and click on "User Defined Weather" and then "Customized Weather" Change the visibility to 20mi / 32km and you're have a nice realistic atmosphere.
2. Get a decent VFR craft. Flightsim has so many different opportunities for creating GA flights that in my opinion, flying low is more far more realistic than flying high. You need something with a good VC, and if you want to keep things real, stay in the VC view mode for the entire flight. I suggest any Carenado plane for this, or the FSNORDIC Maule. It is the glass windows in the cockpit that make the outside appearance most realistic for me (see below), so bear than in mind when planning a flight.

3. Get some addons to enhance your environment below you. I strongly recommend VOZ 1.1 which has new textures for Australia, but work great all over the Southern Hemisphere. The VOZ waters also reflect clouds and sunlight, which is fantastic considering it is freeware. Mesh is also a necessity for enhancing hillsides and landscapes. It makes your flight much realistic when turbulence is turned on in the realism settings too.
4. Speed- you don't need to go fast to enjoy a flight. I usually cruise at around 105-125 kias, which is perfect for slower machines (like mine) as your ground textures don't blur. Also, try not to use autopilot, and have your hand on the yoke the whole time. The more your participate with the controls, the more realistic your flight should feel.
5. Time of day is of upper most importance too. To get the best results, set your Time/Date settings to dawn, then press the up arrow until the time just changes to daytime. This depends on what season you are using, but 7am is great. This way, you have the sun low in the sky, reflecting of all your autogen buildings and creating lovely shadows over hillsides and valleys.
Now you may disagree with me, or maybe everything I have said is very basic information, but I just thought I would share what works for me, with you, as at the moment I am loving flying in my virtual world. B)