The biggest upgrade to my system was the installation of passive acoustic treatments.
Pre-2013, when I had vey little appreciation of the importance of room acoustics, the way in which my room was furnished made it a pretty decent sounding room, though this was entirely by accident and not design! I had a huge bank of wardrobes, two seater sofa, and four unused IMF transmission line loudspeakers occupying the corners that were inadvertently acting as bass traps.
Turning this room into a dedicated listening room and reclaiming square footage in the process, I removed all of the aforementioned clutter. This had dire consequences. I was utterly dejected when I realised how poor my hifi now sounded. TV speech in particular had deteriorated to the point of complete unintelligibility, a smeared, resonant, boomy mess. I dread to think how worse it would have been with bare floors (thankfully I retained the carpet!).
Installing GIK 244 absorption panels at first reflection points on the side walls helped to restore some of the focus/clarity, but the biggest improvement was filling every corner of the room with GIK Tri-Traps running floor to ceiling. This really got the low frequency decay times back under control, reducing my RT60 from 0.7 seconds to 0.3 seconds for all frequencies above 80Hz, making everything sound clearer, more agile and dynamic.
I still have bass issues below 100Hz, as do most listeners with typical UK-sized rooms. These are incredibly difficult to treat with broadband acoustic absorbers unless you sacrifice a significant % of your room's volume to them. Tuned membrane and Helmholtz resonators are more effective at targeting problem modal frequencies, and these are something I'd like to experiment with at some point, together with a first reflection ceiling cloud and some diffusion, but my room isn't really big enough or structurally designed in a way that could accommodate everything that's been recommended to me (and neither is my wallet!).
Thus I have settled for a combination of 1) the passive treatments I currently have; 2) optimising the listening position and loudspeaker position to minimise the remaining issues; and 3) using digital parametric EQ to take the edge off the peaks in the response caused by my axial room modes). I'm currently very content with this compromise.
EDIT - If I were doing my room treatments again I would probably choose corner traps faced with diffusers, as I have since read that, unlike primary-reflection absorption, the absorption of secondary reflections is not necessarily desirable as it can over-damp high-frequencies and thus reduce "room ambience". In some modern houses though with tiled-flooring, stretches of glazed walls, glass coffee tables and leather seating I suspect you'd want all the primary and secondary absorption you could get from passive treatments!