You guys really should have tested the OEM standards as well, a big one would be Shin-Etsu X23-7783D, odds are if you buy a decent heat sink, that's likely what's on it. You should have tested some phase change materials as well. Unfortunately, you really need to buy the sealed can and not the stuff in syringes as X23 uses a volatile solvent to reduce application viscosity and when you buy it as a syringe, that solvent will be gone and the viscosity won't be the same. Anyway, most of the consumer grade TIMs are based on marketing gimmicks rather than actual thermal performance (e.g. silver filled compounds and their bulk thermal conductivity values).
In the case of thermal greases, thermal conductivity of the filler particles isn't as important as bond line thickness. This is why your liquid metal solutions did so well, the bond line thickness in those cases are typically limited by tolerances and material viscosity. This is also why things like silver filled compounds don't do as well as people think they should based on bulk thermal conductivity values as bulk thermal conductivity isn't as important in thin bond line applications as interfacial thermal resistance and particle size are. Silver compounds tend to be rather large and flaky so they don't lend themselves well to low viscosities, ease of processing, or thin bond lines.
I've seen other suggestions here too about using diamond. We've played with those but diamond has lots of issues with it, namely phonon scattering and processing difficulty. Alumina is already harsh enough of mixing vessels and pumping/dispensing systems, diamond would be even worse, so I doubt there will ever be any serious industry production. There will likely be some small 'garage' companies that make diamond filled TIMs but phonon scattering seems to be a major factor in decreasing the thermal performance and making it such that it doesn't perform any better than AlN, ATH or alumina, despite diamonds obscenely high thermal conductivity.
Similarly, graphite, despite having a very high TC, doesn't work as well as you'd think either. Graphite has a very high thermal conductivity, in the x-y plane, but the z plane is extremely low. To combat this, the particles are made into conglomerates with random z-axis orientation which results in the overall thermal conductivity not being much greater than that of standard fillers, also conglomerates like to break up in mixing, adding more complications. Graphite does have fairly small particle size though, making for great bond line thickness, however that also means the surface area to volume ratio is very high, resulting in a very high viscosity relative to filler loading which serves to fight against going to a small bond line at low pressures.
I would also like to caution people regarding liquid metal. DO NOT USE LIQUID METAL ON ALUMINUM. The liquid metals used in TIMs will dissolve aluminum over time (aluminum is soluble in the liquid metal), you can only use liquid metal TIMs on copper heat sinks, the heat spreaders on CPUs are typically copper coated with nickel and that is okay too. The other issue with liquid metals is they like to separate from the silicone carrier so you can end up with 'gobs' of liquid metal separating out from the TIM over time.