As the astute denizens of this site have already pointed out, keeping His commandments is surely the most central way to follow the greatest commandment.
I will divulge how I have failed to keep this great commandment and we can contrast. Below are a list of ways I have failed--
1) Failing to trust God. To trust his plans and timing.
2) Feeling like His will isnt enough. Trying to have my way instead.
3) Breaking the commandment of loving thy neighbor as thyself. The second greatest commandment is related to the first.
4) Being fretful, anxious, fearful of the future. Indicating a lack of trust and peace.
5) Seeking alternative or worldly passions and joys instead of making God the source of all my joy and peace.
6) Being angry or irritated with God. Feeling like God owes me something.
7) Seeking out the world, the pride of life.
8) Failing to apply the teachings of his word in daily life. Being a forgetful hearer and giving in to my desires.
Not to worry, Friend Of. The part I haven't gotten to yet is that the demand of this commandment is, in my opinion, extremely high. It's so high that I think this is why it singly gets overlooked. Certainly He is a God of grace, but what He calls us to and what He wants in asking for our whole heart, mind, soul and strength cam leave one a little despondent for failing Him in so many ways.
I could list all my failings as well. I am not there yet at all. But I see fully grasping His expectations and how far I still have to go as progress. To me this is far better than just thinking I'm the next best thing to sliced bread when I'm nowhere near walking in the kind of godliness and devotion to Him He has asked all His people to walk in.